Photo-induced modification and relaxation dynamics of Weyl-semimetals

The use of ultrashort laser pulses to investigate the response of materials on femtosecond time-scales enables detailed tracking of charge, spin and lattice degrees of freedom. When pushing the limits of the experimental resolution, connection to theoretical modeling becomes increasingly important in order to infer causality relations. Weyl-semimetals is particular class of materials of recent focus due to the topological protection of the Weyl-nodes, resulting in a number of fundamentally interesting phenomena. In this work, we provide a first-principles framework based on time-dependent density-functional theory for tracking the distribution of Weyl-nodes in the Brillouin-zone following an excitation by a laser pulse. For the material TaAs, we show that residual shifts in the Weyl-Nodes' position and energy distribution is induced by a photo-excitation within femto-seconds, even when the laser-frequency is off-resonant with the Weyl-node. Further, we provide information about the relaxation pathway of the photoexcited bands through lattice vibrations

Itinerant magnetic multipole moments of rank five, triakontadipoles, as the hidden order in URu2_{2}Si2_{2}

A broken symmetry ground state without any magnetic moments has been calculated by means of local-density-approximation to density functional theory plus a local exchange term, the so-called LDA+$U$ approach, for URu$_{2}$Si$_{2}$. The solution is analysed in terms of a multipole tensor expansion of the itinerant density matrix and is found to be a non-trivial magnetic multipole. Analysis and further calculations show that this type of multipole enters naturally in time reversal breaking in presence of large effective spin-orbit coupling and co-exists with magnetic moments for most magnetic actinidesComment: 5 pages, 3 figure

Multipole decomposition of LDA+UU energy and its application to actinides compounds

A general reformulation of the exchange energy of $5f$-shell is applied in the analysis of the magnetic structure of various actinides compounds in the framework of LDA+U method. The calculations are performed in an efficient scheme with essentially only one free parameter, the screening length. The results are analysed in terms of different polarisation channels, due to different multipoles. Generally it is found that the spin-orbital polarisation is dominating. This can be viewed as a strong enhancement of the spin-orbit coupling in these systems. This leads to a drastic decrease in spin polarisation, in accordance with experiments. The calculations are able to correctly differentiate magnetic and non-magnetic Pu system. Finally, in all magnetic systems a new multipolar order is observed, whose polarisation energy is often larger in magnitude than that of spin polarisation.Comment: Fixed some references and picture

A route towards finding large magnetic anisotropy in nano-composites: application to a W1−x_{1-x}Rex_x/Fe multilayer

We suggest here a novel nano-laminate, 5[Fe]/2[W$_x$Re$_{1-x}$] (x=0.6-0.8), with enhanced magnetic hardness in combination with a large saturation moment. The calculated magnetic anisotropy of this material reaches values of 5.3-7.0 MJ/m$^3$, depending on alloying conditions. We also propose a recipe in how to identify other novel magnetic materials, such as nano-laminates and multilayers, with large magnetic anisotropy in combination with a high saturation moment

Optically controlling the competition between spin flips and intersite spin transfer in a Heusler half-metal on sub-100 fs timescales

The direct manipulation of spins via light may provide a path toward ultrafast energy-efficient devices. However, distinguishing the microscopic processes that can occur during ultrafast laser excitation in magnetic alloys is challenging. Here, we study the Heusler compound Co2MnGa, a material that exhibits very strong light-induced spin transfers across the entire M-edge. By combining the element-specificity of extreme ultraviolet high harmonic probes with time-dependent density functional theory, we disentangle the competition between three ultrafast light-induced processes that occur in Co2MnGa: same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafast spin-flips mediated by spin-orbit coupling. By measuring the dynamic magnetic asymmetry across the entire M-edges of the two magnetic sublattices involved, we uncover the relative dominance of these processes at different probe energy regions and times during the laser pulse. Our combined approach enables a comprehensive microscopic interpretation of laser-induced magnetization dynamics on timescales shorter than 100 fs.Comment: 31 pages, 12 figure

Theoretical Studies of Magnetism and Electron Correlation in Solids

This work presents new development and applications of ab-initio simulation tools for material science. Focus lies on materials with strong electronic correlation and strong spin-orbit coupling. Improvements on methods for solving the impurity problem in LDA+DMFT is presented, as well as a reliant method for charge self-consistency in a LMTO based electronic structure code. A new adaptive scheme for Brillouin zone integration is developed, where we show a strong reduction of numerical noise compared to standard techniques. A reformulation of the standard LDA+U method aiming to reduce the number of free parameters is introduced. Fast and realistic reduction of the number of free parameters provides the possibility of high throughput calculations and enabled us to study a large number of compounds. An analysis method for polarization in terms of coupled multipoles, and their corresponding energy contributions is developed and applied. This led to the formulation of Katt's rules, a set of rules complementary to Hund's rules. Katt's rules applies for occupying the orbitals of an electronic shell with strong spin-orbit coupling. The analysis is also used to investigate the unconventional Uranium based superconductors URu2Si2, UPt3, UPd2Al3 and UNi2Al3, as well as the high temperature superconductor LaOFeAs. We also investigate the non-magnetic delta-phase of Plutonium, providing insight to the electronic structure and the branching ratios of 4d to 5f transitions seen in photo emission spectra.The influence of surface reconstruction on the magneto crystalline anisotropy is investigated in multilayer Fe/ZnSe, showing that Fe deposited on an unreconstructed interface strongly reduces the uniaxial component of the MAE. We provide a detailed understanding of the magnetic properties of Fe2P, opening possible routes for enhancing the MAE in this system. A general route to strong MAE in nano-laminates is presented, we apply this to propose a candidate with extremely strong anisotropy energy density, 5Fe/2W1-xReX for x=[0.6-0.8]

Theoretical Studies of Magnetism and Electron Correlation in Solids

This work presents new development and applications of ab-initio simulation tools for material science. Focus lies on materials with strong electronic correlation and strong spin-orbit coupling. Improvements on methods for solving the impurity problem in LDA+DMFT is presented, as well as a reliant method for charge self-consistency in a LMTO based electronic structure code. A new adaptive scheme for Brillouin zone integration is developed, where we show a strong reduction of numerical noise compared to standard techniques. A reformulation of the standard LDA+U method aiming to reduce the number of free parameters is introduced. Fast and realistic reduction of the number of free parameters provides the possibility of high throughput calculations and enabled us to study a large number of compounds. An analysis method for polarization in terms of coupled multipoles, and their corresponding energy contributions is developed and applied. This led to the formulation of Katt's rules, a set of rules complementary to Hund's rules. Katt's rules applies for occupying the orbitals of an electronic shell with strong spin-orbit coupling. The analysis is also used to investigate the unconventional Uranium based superconductors URu2Si2, UPt3, UPd2Al3 and UNi2Al3, as well as the high temperature superconductor LaOFeAs. We also investigate the non-magnetic delta-phase of Plutonium, providing insight to the electronic structure and the branching ratios of 4d to 5f transitions seen in photo emission spectra.The influence of surface reconstruction on the magneto crystalline anisotropy is investigated in multilayer Fe/ZnSe, showing that Fe deposited on an unreconstructed interface strongly reduces the uniaxial component of the MAE. We provide a detailed understanding of the magnetic properties of Fe2P, opening possible routes for enhancing the MAE in this system. A general route to strong MAE in nano-laminates is presented, we apply this to propose a candidate with extremely strong anisotropy energy density, 5Fe/2W1-xReX for x=[0.6-0.8]